Abstract: Novel magnetic imprinted polymers are designed by molecular simulation from a comprehensive perspective and prepared rationally by combining the modified surface imprinting technique with the improved atom transfer radical polymerization. The simulation results show that interaction intensity between indole and monomers are simultaneously affected by complex conformation, charge transfer and binding energy. The optimal monomer for the removal of indole is AM and the best ratio is 1 : 4 in the studied three monomers. To verify the reliability and accuracy of the simulation results, three kinds of novel magnetic imprinted polymers are prepared with different monomers. The experimental results show that molecular simulation is reliable in processing the pre-assembled complexes of molecularly imprinted polymers (MIPs). The MIPs using AM as monomer display the highest selectivity (2.561) and bonding percentage (31.062%). Structural superiority of the optimal adsorbent is reflected by using several characterization methods. A series of static adsorption tests such as kinetic, isotherm and selectivity are used to analyse the adsorption performance. The test results show that the novel adsorbents conform to the Elovich kinetic equation and follow the Langmuir isotherm model. Meanwhile, they display higher selectivity towards indole than towards other analogues. The novel adsorbents have potential application value in the denitrogenation fieldTemplate and target information:indole